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嵌入MoS纳米片的UiO-66-NH金属有机框架用于可见光介导的析氢和析氧反应

UiO-66-NH Metal-Organic Frameworks with Embedded MoS Nanoflakes for Visible-Light-Mediated H and O Evolution.

作者信息

Subudhi Satyabrata, Swain Gayatri, Tripathy Suraj Prakash, Parida Kulamani

机构信息

Centre for Nanoscience and Nanotechnology, Siksha 'O' Anusandhan (Deemed to be University), Bhubaneswar, Odisha 751030, India.

出版信息

Inorg Chem. 2020 Jul 20;59(14):9824-9837. doi: 10.1021/acs.inorgchem.0c01030. Epub 2020 Jul 6.

Abstract

Hydrogen evolution from water splitting by means of a photocatalytic approach is an ideal future energy source and free of fossil reserves, in contrary photocatalytic O evolution remains a bottleneck due to high over potential and low efficiency. For reasonable use of solar light, photocatalysts must be sufficiently stable and efficient toward harvesting of sunlight from both theoretical and practical viewpoints. In this regard, here we have prepared MoS-modified UiO-66-NH MOF through a facile hydrothermal technique and evaluated its efficiency toward photocatalytic H and O evolution by water splitting in the presence of sacrificial agents. A couple of similar type of analyses have been studied previously; however, this analysis represents a diverse scientific approach on the basis of interfacial contact toward reveal the actual potential of nanoflakes MoS as well as UiO-66-NH. In this regard the as-synthesized photocatalyst was well-characterized by XRD, FTIR, UV-vis diffuse reflectance spectra, FESEM, HRTEM, XPS, and BET analysis techniques, which provide sufficient evidence toward successful synthesis of the pristine materials and efficacious anchorage of MoS on the active surface of UiO-66-NH by the ionic interaction between Zr-O and S/Mo. Among the synthesized photocatalysts (3 wt %) MoS/UiO-66-NH shows the optimum outcome toward H and O evolution, i.e., 512.9 μmol/h (4.37 times greater than bare UiO-66-NH) and 263.6 μmol/h (4.25 and 11.32 times greater than bare UiO-66-NH and MoS, respectively). The superior performance obtained by the composite is due to the synergistic effect of pristine UiO-66-NH and MoS which proceeds through a type-II interband alignment for the facile channelization of excitons. This investigation will bestow a beneficial blue-print to construct challenging photocatalysts and to find out the paramount performance toward photocatalytic water redox reaction.

摘要

通过光催化方法从水分解中析氢是一种理想的未来能源,且不受化石燃料储备的限制,相反,由于过电位高和效率低,光催化析氧仍然是一个瓶颈。为了合理利用太阳光,从理论和实际角度来看,光催化剂必须对太阳光的捕获具有足够的稳定性和效率。在这方面,我们通过简便的水热技术制备了MoS修饰的UiO-66-NH MOF,并在牺牲剂存在下通过水分解评估了其对光催化析氢和析氧的效率。此前已经进行了一些类似类型的分析;然而,该分析基于界面接触提出了一种不同的科学方法,以揭示纳米片MoS以及UiO-66-NH的实际潜力。在这方面,通过XRD、FTIR、紫外可见漫反射光谱、FESEM、HRTEM、XPS和BET分析技术对合成的光催化剂进行了充分表征,这些技术为原始材料的成功合成以及通过Zr-O与S/Mo之间的离子相互作用将MoS有效锚固在UiO-66-NH的活性表面提供了充分的证据。在合成的光催化剂(3 wt%)中,MoS/UiO-66-NH对析氢和析氧显示出最佳结果,即512.9 μmol/h(比裸UiO-66-NH高4.37倍)和263.6 μmol/h(分别比裸UiO-66-NH和MoS高4.25倍和11.32倍)。复合材料获得的优异性能归因于原始UiO-66-NH和MoS的协同效应,该效应通过II型带间排列进行,以实现激子的便捷通道化。这项研究将为构建具有挑战性的光催化剂以及找出光催化水氧化还原反应的最佳性能提供有益的蓝图。

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